The modification of semiconductor nanostructures with metallic nanocomponents can promote the separation of electron/hole from photoexited semiconductors by forming heterojunctions, thus exhibit enhanced photocatalytic activities and potential applications. In this study, Pt-based NPs, including Pt, PtCu, and PtCuCo are employed as model co-catalysts to comparatively study their capability to enhance the photocatalytic activity of TiO nanosheets. It was found that each of Pt, PtCu, and PtCuCo can greatly enhance the photocatalytic activity of TiO toward degradation of organic dyes. Using electron spin resonance spectroscopy, we demonstrated that deposition of Pt-based NPs resulted in more production of reactive oxygen species including hydroxyl radicals, superoxide, and singlet oxygen. The enhancing effects of Pt-based NPs on generation of ROS and photocatalytic activity showed same trend: PtCuCo > PtCu > Pt. The mechanism underlying the enhancement differences in Pt-based NPs may be mainly related to electronic structure change of Pt in alloying with Cu and Co. These results are valuable for designing hybrid nanomaterials with high photocatalytic efficiency for applications in water purification and antibacterial products.